Novel ethylene diamine tetraacetic acid (EDTA)‐modified zwitterionic hybrid materials were prepared via a sol–gel process. Their adsorption performances for Pb2+ ions were examined. Fourier transform infrared spectroscopy confirmed the reaction products. Thermogravimetric analysis revealed that the thermal stability of these hybrid materials could reach 200°C. Differential scanning calorimetry measurement showed that the addition of titanium butoxide could impact the crystallization transformation of these materials. Field emission scanning electron microscopy images showed that EDTA modification induced a decrease in the particle size. Adsorption experiments demonstrated that the optimal initial pH was 5. Moreover, we observed that the adsorptions for Pb2+ ions followed the Lagergren pseudo‐second‐order kinetic model, intraparticle diffusion, and Langmuir isotherm model. In addition, we found that the maximal Langmuir constant was 0.86 mmol/g. The negative Gibbs free energy values suggested that Pb2+ adsorption onto these samples was spontaneous in nature. The desorption experiment indicated that these samples could be recovered with aqueous HCl solution as a desorbent. These results suggest that the synthesized EDTA‐modified zwitterionic hybrid materials are promising adsorbents that could be used to separate and recover heavy‐metal ions from polluted wastewater. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 39801.